Quantum Size Effect in Optically Active Indium Selenide Crystal Phase Heterostructures Grown by Molecular Beam Epitaxy

Jacek Kossut; Jaroslaw Z. Domagala; Maciej Wojcik; Maksymilian Kuna; Marta Aleszkiewicz; Pawel Ciepielewski; Piotr Baranowski; Piotr Wojnar; Roza Dziewiatkowska; Sergij Chusnutdinow

REVIEW 3 major objections 6 minor 31 references

Quantum Size Effect in Optically Active Indium Selenide Crystal Phase Heterostructures Grown by Molecular Beam Epitaxy

T0 review · 3 major / 6 minor · reviewed 2026-08-15 · deepseek-v4-flash

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Pith's one-line read A 250 meV blueshift ties indium selenide heterostructure emission to a type-II interface transition.

desk verdict Credible MBE-grown InSe phase heterostructures with a tunable interface emission, but the quantitative quantum-size-effect numbers rest on extrapolated thicknesses and a fitted mass. read the letter →

arxiv 2509.06605 v1 pith:OHLAXRSW submitted 2025-09-08 cond-mat.mes-hall

Piotr Wojnar , Maciej Wojcik , Piotr Baranowski , Jacek Kossut , Marta Aleszkiewicz , Jaroslaw Z. Domagala , Roza Dziewiatkowska , Pawel Ciepielewski

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Maksymilian Kuna Zuzanna Kostera Slawomir Kret Sergij Chusnutdinow

This is my paper · ORCID

classification cond-mat.mes-hall PACS 81.15.Hi78.55.-m73.21.-b

keywords indiumselenidecrystalphaseheterostructuresmolecularbeamepitaxyquantumsizeeffecttype-IIbandalignmentphotoluminescencenear-infraredemittersvanderWaalssemiconductors

verification ladder T0 review T1 audit T2 compute T3 formal

The pith

A machine-rendered reading of the paper's core claim, the machinery that carries it, and where it could break.

The reading

The paper reports molecular beam epitaxy growth of indium selenide crystal phase heterostructures, showing that the In/Se flux ratio selects between γ-InSe, γ-In2Se3, and β-In2Se3 phases. It claims that the γ-InSe/γ-In2Se3 interface emits intensely in the near infrared at 1.10 eV, and that shrinking the γ-InSe layer below 20 nm blueshifts this emission by up to 250 meV. This thickness dependence is presented as evidence for a quantum size effect in a type-II staggered band alignment, with the optical transition occurring across the interface. A sympathetic reader would care because it demonstrates a route to large-area, lithographically patternable near-IR light sources and detectors built from a single materials family.

What carries the argument

The argument turns on the type-II (staggered) band alignment at the γ-InSe/γ-In2Se3 interface, which places the electron and hole in different layers so the optical transition energy is lower than either band gap. Quantum confinement in the conduction band of the γ-InSe slab raises the electron level as the layer thins, producing the blueshift; the paper models this as an electron in a potential well with $m_e = 0.09\,m_0$, treating the valence band as unconfined because of the small valence band offset.

What would settle it

Measure the actual thickness of the nominally 5 nm and 8 nm γ-InSe layers by cross-sectional scanning transmission electron microscopy; if the real thicknesses differ enough that the emission energies no longer follow the $0.09\,m_0$ quantum-well curve, the quantum size effect interpretation and derived band offsets would need revision.

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Extended reading notes

Core claim

The central claim is that the 1.10 eV photoluminescence from γ-InSe/γ-In2Se3 is an interface (type-II) transition, not a defect transition. The paper supports this by showing the emission blueshifts by about 250 meV when the γ-InSe layer thickness drops from 20 nm to 5 nm, which matches calculations of a confined electron in a quantum well with effective mass $m_e = 0.09\,m_0$. From the large-thickness emission energy, the paper derives a valence band offset of 0.15 eV and a conduction band offset of 1.04 eV between γ-InSe and γ-In2Se3. It also reports that the emission vanishes below about 5 nm, consistent with a direct-to-indirect band gap crossover in thin γ-InSe.

Load-bearing premise

The thicknesses of the thinnest γ-InSe layers, where the largest blueshift is observed, are not measured directly but extrapolated from growth time using a rate calibrated on layers thicker than 10 nm.

Editorial extensions

If this is right

If the interpretation is right, the emission wavelength of γ-InSe/γ-In2Se3 heterostructures is set by γ-InSe thickness and can be designed from about 1.10 eV to 1.35 eV.
The derived valence band offset (0.15 eV) and conduction band offset (1.04 eV) give a concrete band diagram for further InSe device engineering.
The inability to grow β-In2Se3 on γ-In2Se3 shows that not all phase combinations are kinetically accessible, guiding future phase-heterostructure design.
The quenching of PL below 5 nm marks a thickness window for useful emitters and correlates with the direct-indirect crossover reported for exfoliated InSe.
The linear power dependence and fluence blueshift support an excitonic interface recombination channel.

Reading between the lines

Editorial extensions of the paper, not claims the author makes directly.

The extracted effective mass of $0.09\,m_0$ is likely the out-of-plane (c-axis) electron mass of γ-InSe; one could test it independently with magneto-optical measurements on the same heterostructures.
If thickness can be controlled to the monolayer level, the same quantum size effect could push emission across the near-infrared into the visible, extending the platform beyond the 250 meV range reported.
The phase-selection rule (In/Se flux ratio dominant) suggests that other III-VI compounds with competing polymorphs might support analogous phase heterostructures by the same MBE switching method.
A direct STEM thickness measurement on the thinnest samples would confirm whether the growth-rate extrapolation holds and would sharpen the fitted mass and offsets.

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Editorial analysis

A structured set of objections, weighed in public.

Desk editor's note, referee report, and a circularity audit.

Desk Editor's Note

read the letter

Quick take: this is a credible experimental paper that demonstrates something new—MBE-grown heterostructures between two different indium selenide crystal phases with a sharp interface and thickness-tunable near-infrared emission. The qualitative result (the 250 meV blueshift as the γ-InSe layer thins) is likely correct. The quantitative interpretation (effective mass 0.09 m0, VBO 0.15 eV) is shakier, because it depends on thicknesses that were extrapolated from growth time and a mass fitted to the same data.

What the paper does well: the growth phase diagram is a useful contribution. The authors identify clean windows for γ-InSe, γ-In2Se3, and β-In2Se3 as a function of In/Se ratio and temperature, and they back the phase assignment with Raman, low-temperature PL, XRD, and STEM. The STEM image of the γ-InSe/γ-In2Se3 interface is convincing evidence of an abrupt lattice change. The PL story is also coherent: the 1.10 eV line appears only in the heterostructure, shifts monotonically with thickness, has an excitation-power dependence consistent with a type-II interface transition, and disappears at low thickness in a way consistent with the known direct-to-indirect crossover in thin InSe. That is a solid chain of evidence for an interfacial quantum-confined emission.

The soft spots are real but narrow. The thin-layer thicknesses—exactly the ones that carry the blueshift—are not measured directly; they are extrapolated from growth time using a rate calibrated on layers >10 nm. The RHEED data show the γ-In2Se3-to-γ-InSe conversion takes the first ~3 nm, so the early growth rate may not be constant. A 20–30% error in the thinnest-layer thicknesses would change the fitted mass noticeably. The paper also gives no error bars on the five PL peak positions, and the fit uses one free parameter (me) after fixing VBO from the thick-layer emission energy. None of this threatens the existence of the size effect—the blueshift with growth time is monotonic and qualitative—but it does mean the quoted mass and band offsets should be treated as rough estimates, not precise values.

One more minor point: the abstract says 'β-yIn2Se3' which looks like a typo, and the Conclusions say the temperature range is 350–400 °C while the phase diagram covers 300–450 °C. Small inconsistencies, easily fixed.

Who this is for: experimentalists working on van der Waals epitaxy, 2D optoelectronics, and InSe-based devices. It is a good paper to referee seriously. I would send it to review, with the request that the authors add a direct thickness measurement or at least discuss the early-nucleation uncertainty, and include error bars on the PL energies. The qualitative advance is worth publishing; the quantitative model needs a caveat.

Referee Report

3 major / 6 minor

Summary. The manuscript reports MBE growth of indium selenide in different crystal phases (γ-InSe, γ-In2Se3, β-In2Se3) by controlling the In/Se flux ratio, and uses this control to fabricate γ-InSe/γ-In2Se3 phase heterostructures. The central experimental finding is an intense near-infrared emission near 1.10 eV from these heterostructures, attributed to a type-II interface transition. The authors show that this emission blueshifts by up to 250 meV when the γ-InSe layer thickness is reduced from tens of nanometers to about 5 nm, and they interpret this blueshift as a quantum size effect. A calculation with a one-parameter fit for the electron effective mass (me = 0.09 m0) and a valence band offset inferred from the thick-layer emission energy (VBO = 0.15 eV) is said to reproduce the thickness dependence. The paper also presents temperature- and excitation-power-dependent PL measurements supporting the type-II interface assignment.

Significance. If the quantitative interpretation is upheld, this is a valuable demonstration of MBE-grown, all-indium-selenide phase heterostructures with an interface emission tunable over a practically relevant near-infrared range. The qualitative claim—that the emission energy depends strongly on the γ-InSe layer thickness—is well supported by the measured thickness series, the absence of such a shift for thick layers, and the consistency of temperature and power dependence with a type-II transition. The paper's strengths include the multi-technique phase identification (Raman, PL, XRD, RHEED, STEM, AFM), the direct STEM evidence of an abrupt γ-InSe/γ-In2Se3 interface, and the explicit demonstration that the emission is not the ordinary γ-InSe band-edge transition. The main load-bearing weakness is the quantitative modeling: the thin-layer thicknesses are extrapolated from growth time, and the effective mass is fitted to the same data the model explains, so the numerical values (0.09 m0 and 0.15 eV) are less robust than the qualitative confinement effect.

major comments (3)

[Section 2.3, Fig. 3c] The quantitative QSE calculation is anchored to a thickness axis that is explicitly extrapolated from growth time for the thinnest layers—precisely the layers (5 and 7 nm) that carry the 250 meV blueshift. Because the growth sequence includes a 30 min interruption and a change of Se flux, and RHEED shows that the phase conversion is not complete until after about 3 nm of growth, an early-growth-rate transient cannot be excluded. A systematic thickness error of 20–30% would materially change the fitted value me = 0.09 m0 and the inferred VBO = 0.15 eV. The authors should provide direct thickness measurements for at least the thinnest samples (e.g., STEM cross-sections) or a sensitivity analysis showing how the fitted parameters depend on assumed thickness errors, and they should include error bars on the data points in Fig. 3c.
[Section 2.3, VBO derivation] The valence band offset is obtained as VBO = Eg2 − Ed = 0.15 eV, treating the thick-layer emission energy as exactly equal to Eg2 − VBO. This neglects the exciton binding energy of the spatially separated electron-hole pair at the type-II interface, possible strain-related shifts (which the authors themselves invoke in Sec. 2.1 to explain the 1.23 eV emission of γ-InSe on GaAs), and any residual confinement at 30–65 nm. The inferred VBO should therefore be presented with an estimated uncertainty or as an approximate value, rather than as the definitively determined offset stated in the Conclusions.
[Section 2.3, Fig. 3c model] The model calculation uses me = 0.09 m0 as the single fitted parameter and VBO derived from the same experimental data set. The paper does not provide raw data points, fit residuals, or a discussion of the parameter sensitivity. As presented, the statement that the blueshift is 'well reproduced by the calculations' is a one-parameter fit to five points whose abscissae carry unquantified uncertainty. Please show the individual PL spectra or extracted peak positions for all five thicknesses, report the fit residuals, and clarify which aspects of the fit are robust (e.g., the functional form of the confinement shift) versus parameter-dependent.

minor comments (6)

[Abstract] The abstract contains the typo 'β-yIn2Se3'; this should read 'β-In2Se3'.
[Fig. 1d caption] The caption refers to 'indium telluride thin layers' but the paper is about indium selenide; this should be corrected.
[Section 2.3 and Fig. 4] The text and figure captions use 'fluence of 0.5 mW' and '30 mW', but milliwatts are units of power, not fluence. Please use consistent units (e.g., W/cm² or report the spot size and power) and refer to excitation power where appropriate.
[Conclusions vs. Section 2.1] The Conclusions state that growth temperature variation 'in the range 350–400 °C' affects surface roughness, but Section 2.1 and Fig. 1a describe the range 300–450 °C; these statements should be reconciled.
[Section 2.3] The paper mentions a 'comprehensive study involving scanning electron microscopy of the structure cross-section' for thickness calibration, but no SEM images or calibration curve are shown. Adding a representative SEM cross-section and the growth-rate calibration data would make the extrapolation procedure transparent.
[References] Reference [30] has an incomplete author name ('G. S˛'); the full author list should be provided.

Circularity Check

0 steps flagged · score 0.0 of 10

No circularity: the thickness-dependent blueshift is an independent measurement; VBO and electron mass are openly fitted calibration inputs, not predictions, and the type-II alignment comes from external literature.

full rationale

The paper's central claim is the measured 250 meV blueshift of the 1.10 eV emission as the gamma-InSe layer thickness decreases below 20 nm. The quantum-size-effect calculation in Section 2.3 is not circular: the VBO is calibrated from the thick-layer emission energy (VBO = Eg2 - Ed = 0.15 eV), and the electron effective mass me = 0.09 m0 is a best fit to the same thickness series, but the thickness dependence itself is an independent experimental observable that is not forced by these calibrations. The type II band alignment is adopted from an external reference (ref. [13], Balakrishnan et al.), not from the authors' own prior work, and no uniqueness theorem or self-citation chain is invoked. The extrapolation of the thinnest-layer thicknesses from growth time is an experimental uncertainty that could affect the quantitative fit, but it is not a definitional equivalence or a fitted parameter renamed as a prediction. The paper explicitly presents the mass as a fit and the blueshift as reproduced rather than as an independent prediction, so there is no step in which an output reduces by construction to an input.

Assumptions & free parameters 1 free parameters · 4 assumptions · 0 invented entities

The central interpretation rests on the type II band alignment taken from prior literature, the assumption that only electrons are confined, literature band gaps, and extrapolated thin-layer thicknesses. The only number fitted to the data is the electron effective mass; the valence band offset is derived from the measured thick-layer emission and the assumed InSe gap.

free parameters (1)

electron effective mass in gamma-InSe (me) = 0.09 m0
Chosen as the best fit to the experimental thickness-dependent blueshift in Figure 3c; not independently measured.

assumptions (4)

domain assumption gamma-InSe and gamma-In2Se3 form a staggered (type II) band alignment with a small valence band offset and a large conduction band offset.
Invoked in Section 2.3 and the inset of Figure 3c, citing reference [13]; the interface emission model depends on this alignment.
domain assumption Quantum confinement acts only on electrons in the gamma-InSe conduction band, with holes unconfined, and the confinement is approximated by an infinite potential well.
Used in Section 2.3 to compute the blueshift; if holes also confine, the fitted effective mass and inferred VBO would change.
domain assumption The band gaps used in the model are Eg(gamma-In2Se3) = 2.14 eV and Eg(gamma-InSe) = 1.25 eV, taken from prior literature.
Used to convert the measured 1.10 eV thick-layer emission into VBO = 0.15 eV; uncertainties in these values propagate into VBO.
domain assumption The gamma-InSe layer thickness for the thinnest samples equals growth time times a constant growth rate calibrated on thicker layers.
Section 2.3 states thin-layer thicknesses are extrapolated from growth time; if the growth rate drifts, the thickness axis and the quantum-size-effect fit are affected.

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Cite this review

Pith. "Pith review of Quantum Size Effect in Optically Active Indium Selenide Crystal Phase Heterostructures Grown by Molecular Beam Epitaxy." pith.science (2026). https://pith.science/paper/OHLAXRSW

@misc{pith2026250906605,
  author       = {Pith},
  title        = {Pith review of: Quantum Size Effect in Optically Active Indium Selenide Crystal Phase Heterostructures Grown by Molecular Beam Epitaxy},
  year         = {2026},
  howpublished = {\url{https://pith.science/paper/OHLAXRSW}},
  note         = {Machine review of arXiv:2509.06605}
}

read the original abstract

Indium selenide attracts the interest due to its outstanding electronic and optical properties which are potentially prospective in view of applications in electronic and photonic devices. Most of the polymorphic crystal phases of this semiconductor belong to the family of two-dimensional van der Waals semiconductors. In this study optically active indium selenide crystal phase heterostructures are fabricated by molecular beam epitaxy in a well-controlled manner. It is demonstrated that by changing the growth conditions one may obtain either {\gamma}-InSe, or {\gamma}-In2Se3, or \b{eta}-yIn2Se3 crystal phases. The most promising crystal phase heterostructures from the point of view of photonic applications is found to be the {\gamma}-InSe/{\gamma}-In2Se3 heterostructure. An intense optical emission from this heterostructure appears in the near infrared spectral range. The emission energy can be tuned over 250 meV by changing {\gamma}-InSe layer thickness which is explained by the quantum size effect. The optically active indium selenide crystal phase heterostructures represent, therefore, an interesting platform for the design of light sources and detectors in the near infra-red. The use of molecular beam epitaxy for this purpose ensures that the structures are fabricated on large surfaces opening the possibility for the design of device prototypes by using lithography methods

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Pith tools

Reviewed August 15, 2026 · model on record in the stance chip above.

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